Research ArticleMATERIALS SCIENCE

Bilateral alkylamine for suppressing charge recombination and improving stability in blade-coated perovskite solar cells

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Science Advances  08 Mar 2019:
Vol. 5, no. 3, eaav8925
DOI: 10.1126/sciadv.aav8925
  • Fig. 1 Chemical structures and functions of BAA additives, contact angle measurement, and blading process.

    (A) Chemical structures of BAA additives. (B) Schematic illustration of defect passivation and water repellence induced by BAA incorporation. (C) Contact angle measurement of a water droplet on MAPbI3 single crystals (top row) and MAPbI3 thin films (bottom row) with or without incorporated BAA additive. Scale bars, 5 cm. (D) Sketch showing the blade-coating process for the perovskite film.

  • Fig. 2 Perovskite film morphologies and mechanical test.

    Surface SEM images of (A and B) MAPbI3 and (C and D) MAPbI3-DAP (0.025 wt % DAP added). (E) Sketch showing the morphology change of the perovskite films deposited on a flexible ITO-PET substrate after the bending test. Corresponding SEM images of (F) MAPbI3 and (G) MAPbI3-DAP films after bending. (H) SEM images showing the degradation of grain boundaries for MAPbI3 and MAPbI3-DAP films after exposure to the high energy electron beam for several scanning cycles during SEM characterization. Scale bar, 500 nm (H).

  • Fig. 3 Device structure and photovoltaic performance.

    (A) Schematic illustration of a completed PSC with inverted p-i-n device structure. (B) J-V curves of PSCs based on different perovskite compositions incorporated with or without DAP additive. (C) Stabilized Voc of MAPbI3-DAP device as a function of time. (D) Stabilized current density and PCE at the maximum power point (0.98 V) of the champion MAPbI3-DAP device (0.08 cm2). (E) PCE histogram of PSCs based on MAPbI3 and MAPbI3-DAP films (with 0.025 wt % DAP). (F) J-V characteristic of the champion 1.1 cm2 PSC based on MAPbI3-DAP thin film (inset shows a digital image of the actual device).

  • Fig. 4 Carrier recombination lifetime, trap densities, ideal factor, and weak light photovoltaic response.

    (A) TRPL of perovskite film incorporated with or without DAP amine. (B) Carrier recombination lifetime measured by transient photovoltage (TPV) and (C) trap density of states (tDOS) obtained from thermal admittance spectroscopy (TAS) measurement of PSCs with or without DAP passivation. (D) Voc and (E) FF dependence as a function of light intensity. (F) J-V curves of PSCs based on MAPbI3-DAP film measured under illumination at different light intensities.

  • Fig. 5 Stability test.

    (A) Moisture stability of nonencapsulated PSCs based on MAPbI3-DAP and MAPbI3 films under ambient air (50 ± 5 RH% at room temperature). (B) Operational stability of encapsulated PSCs based on MAPbI3-DAP and MAPbI3 films under continuous 1-sun illumination.

  • Table 1 Photovoltaic parameters of the PSCs using different perovskite layers prepared with various compositions and ink formulations under 1-sun illumination (AM1.5G, 100 mW cm−2).

    Note that CFM has an optical bandgap of 1.51 eV, MAPbI3 has an optical bandgap of 1.55 eV, and CFPbIBr has an optical bandgap of 1.82 eV. The optical bandgap of perovskite with different composition is determined from the external quantum efficiency (EQE) spectrum edge in figs. S11 to S13. Data for average PCE (η) were calculated from at least 30 devices. CFM represents Cs0.05FA0.70MA0.25PbI3 and CFPbIBr represents Cs0.2FA0.8Pb(I0.6Br0.4)3 (see details in Materials and Methods section).

    PSCsJsc
    (mA cm−2)
    Voc
    (V)
    η
    (%)
    Average η
    (%)
    FF
    (%)
    Voc deficit
    (V)
    CFM23.41.0617.015.02 ± 0.7868.40.45
    CFM-DAP23.41.1621.520.36 ± 0.4679.40.35
    MAPbI322.01.0818.316.45 ± 0.4077.20.47
    MAPbI3-DAP22.51.1821.720.53 ± 0.3881.70.37
    MAPbI3-DAP (1.1 cm2)22.01.1420.018.24 ± 0.6580.0N/A
    CFPbIBr15.11.1813.111.78 ± 0.5773.30.64
    CFPbIBr-DAP15.61.2615.213.87 ± 0.4977.50.56

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/5/3/eaav8925/DC1

    Fig. S1. FTIR measurement of amine-incorporated perovskite material.

    Fig. S2. XRD patterns of perovskite films before annealing.

    Fig. S3. Variation of MAPbI3 film morphology with increasing DAP contents.

    Fig. S4. Effect of different amounts of DAP on perovskite crystal orientation.

    Fig. S5. Surface roughness of perovskite films.

    Fig. S6. Dark current measurement.

    Fig. S7. Energy diagram of PSC device.

    Fig. S8. Perovskite film thickness and quality.

    Fig. S9. Hysteresis study.

    Fig. S10. Lateral device architecture and its current response.

    Fig. S11. EQE measurement of CFM device.

    Fig. S12. EQE measurement of the champion MAPbI3-DAP device.

    Fig. S13. EQE measurement of CFPbIBr-DAP device.

    Fig. S14. Steady PL measurement of perovskite films with different compositions.

    Fig. S15. Carrier recombination lifetime.

    Fig. S16. Light intensity–dependent J-V performances.

    Fig. S17. Stabilized PCE output.

    Fig. S18. Perovskite films degradation in ambient air.

    Fig. S19. Thermal stability test.

    Table S1. Summarized work functions, valence band maximum (VBM), and conduction band minimum (CBM) positions for different functional layers in the PSCs.

    Table S2. Photovoltaic parameters of PSCs using bladed MAPbI3 films incorporated with different amounts of DAP amine additives.

    Table S3. Photovoltaic parameters of PSCs based on MAPbI3-DAP film measured under AM1.5G illumination in different scan directions.

  • Supplementary Materials

    This PDF file includes:

    • Fig. S1. FTIR measurement of amine-incorporated perovskite material.
    • Fig. S2. XRD patterns of perovskite films before annealing.
    • Fig. S3. Variation of MAPbI3 film morphology with increasing DAP contents.
    • Fig. S4. Effect of different amounts of DAP on perovskite crystal orientation.
    • Fig. S5. Surface roughness of perovskite films.
    • Fig. S6. Dark current measurement.
    • Fig. S7. Energy diagram of PSC device.
    • Fig. S8. Perovskite film thickness and quality.
    • Fig. S9. Hysteresis study.
    • Fig. S10. Lateral device architecture and its current response.
    • Fig. S11. EQE measurement of CFM device.
    • Fig. S12. EQE measurement of the champion MAPbI3-DAP device.
    • Fig. S13. EQE measurement of CFPbIBr-DAP device.
    • Fig. S14. Steady PL measurement of perovskite films with different compositions.
    • Fig. S15. Carrier recombination lifetime.
    • Fig. S16. Light intensity–dependent J-V performances.
    • Fig. S17. Stabilized PCE output.
    • Fig. S18. Perovskite films degradation in ambient air.
    • Fig. S19. Thermal stability test.
    • Table S1. Summarized work functions, valence band maximum (VBM), and conduction band minimum (CBM) positions for different functional layers in the PSCs.
    • Table S2. Photovoltaic parameters of PSCs using bladed MAPbI3 films incorporated with different amounts of DAP amine additives.
    • Table S3. Photovoltaic parameters of PSCs based on MAPbI3-DAP film measured under AM1.5G illumination in different scan directions.

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